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We report an unusual canted magnetism due to 3d and 4f electrons, occupyingtwo different crystallographic sites, with its consequence to electric dipoleorder. This is based on neutron powder diffraction measurements on Tb2BaNiO5(orthorhombic, Immm centrosymmetric space group), exhibiting Neel order below(TN) 63 K, to understand multiferroic behavior below 25 K. The magneticstructure is made up of Ni and Tb magnetic moments, which are found to bemutually canted in the entire temperature range below TN, though collinearityis seen within each sublattice, as known in the past. First-principles densityfunctional theory calculations (GCA plus SO and GCA plus U plus SOapproximations) support such a canted ground state. The intriguing finding,being reported here, is that there is a sudden increase in this Tb-Ni relativecantingle angle at the temperature (that is, at 25 K) at which spontaneouselectric polarization sets in, with bond distance and bong angle anomalies.This finding emphasizes the need for a new spin-driven polarization mechanism,that is, a critical canting angle coupled with exchangestriction, to inducemultiferroicity in magnetic insulators with canted spins.

Existence of a critical canting angle of magnetic moments to induce multiferroicity in the Haldane spin-chain system, Tb2BaNiO5